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高温下氨的紫外吸收截面用于燃烧环境中的非侵入式定量检测

Ultraviolet Absorption Cross-Sections of Ammonia at Elevated Temperatures for Nonintrusive Quantitative Detection in Combustion Environments.

作者信息

Weng Wubin, Li Shen, Aldén Marcus, Li Zhongshan

机构信息

Division of Combustion Physics, 5193Lund University, Lund, Sweden.

出版信息

Appl Spectrosc. 2021 Sep;75(9):1168-1177. doi: 10.1177/0003702821990445. Epub 2021 Feb 2.

DOI:10.1177/0003702821990445
PMID:33464157
原文链接:https://pmc.ncbi.nlm.nih.gov/articles/PMC8446901/
Abstract

Ammonia (NH) is regarded as an important nitrogen oxides (NOx) precursor and also as an effective reductant for NOx removal in energy utilization through combustion, and it has recently become an attractive non-carbon alternative fuel. To have a better understanding of thermochemical properties of NH, accurate in situ detection of NH in high temperature environments is desirable. Ultraviolet (UV) absorption spectroscopy is a feasible technique. To achieve quantitative measurements, spectrally resolved UV absorption cross-sections of NH in hot gas environments at different temperatures from 295 K to 590 K were experimentally measured for the first time. Based on the experimental results, vibrational constants of NH were determined and used for the calculation of the absorption cross-section of NH at high temperatures above 590 K using the PGOPHER software. The investigated UV spectra covered the range of wavelengths from 190 nm to 230 nm, where spectral structures of the transition of NH in the umbrella bending mode, , were recognized. The absorption cross-section was found to decrease at higher temperatures. For example, the absorption cross-section peak of the (6, 0) vibrational band of NH decreases from ∼2 × 10 to ∼0.5 × 10 cm/molecule with the increase of temperature from 295 K to 1570 K. Using the obtained absorption cross-section, in situ nonintrusive quantification of NH in different hot gas environments was achieved with a detection limit varying from below 10 parts per million (ppm) to around 200 ppm as temperature increased from 295 K to 1570 K. The quantitative measurement was applied to an experimental investigation of NH combustion process. The concentrations of NH and nitric oxide (NO) in the post flame zone of NH-methane (CH)-air premixed flames at different equivalence ratios were measured.

摘要

氨(NH₃)被视为一种重要的氮氧化物(NOₓ)前驱体,同时也是通过燃烧在能源利用中去除NOₓ的有效还原剂,并且它最近已成为一种有吸引力的无碳替代燃料。为了更好地理解NH₃的热化学性质,需要在高温环境中对NH₃进行准确的原位检测。紫外(UV)吸收光谱法是一种可行的技术。为了实现定量测量,首次在295 K至590 K的不同温度下,对热气体环境中NH₃的光谱分辨紫外吸收截面进行了实验测量。基于实验结果,确定了NH₃的振动常数,并使用PGOPHER软件计算590 K以上高温下NH₃的吸收截面。所研究的紫外光谱覆盖了190 nm至230 nm的波长范围,其中识别出了NH₃在伞形弯曲模式下ν₃跃迁的光谱结构。发现吸收截面在较高温度下会减小。例如,随着温度从295 K升高到1570 K,NH₃的(6, 0)振动带的吸收截面峰值从约2×10⁻²⁰ cm²/molecule降至约0.5×10⁻²⁰ cm²/molecule。利用获得的吸收截面,在不同热气体环境中实现了NH₃的原位非侵入式定量,随着温度从295 K升高到1570 K,检测限从低于百万分之十(ppm)变化到约200 ppm。该定量测量应用于NH₃燃烧过程的实验研究。测量了不同当量比下NH₃ - 甲烷(CH₄) - 空气预混火焰后火焰区中NH₃和一氧化氮(NO)的浓度。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/181f/8446901/63b4b27c8e57/10.1177_0003702821990445-fig6.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/181f/8446901/b90720e3ea64/10.1177_0003702821990445-img1.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/181f/8446901/f56d3dc84d0e/10.1177_0003702821990445-fig1.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/181f/8446901/8b835b77679e/10.1177_0003702821990445-fig2.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/181f/8446901/b694a43fa831/10.1177_0003702821990445-fig3.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/181f/8446901/2aeeb67c74a0/10.1177_0003702821990445-fig4.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/181f/8446901/09016dd8fe6d/10.1177_0003702821990445-fig5.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/181f/8446901/63b4b27c8e57/10.1177_0003702821990445-fig6.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/181f/8446901/b90720e3ea64/10.1177_0003702821990445-img1.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/181f/8446901/f56d3dc84d0e/10.1177_0003702821990445-fig1.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/181f/8446901/8b835b77679e/10.1177_0003702821990445-fig2.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/181f/8446901/b694a43fa831/10.1177_0003702821990445-fig3.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/181f/8446901/2aeeb67c74a0/10.1177_0003702821990445-fig4.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/181f/8446901/09016dd8fe6d/10.1177_0003702821990445-fig5.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/181f/8446901/63b4b27c8e57/10.1177_0003702821990445-fig6.jpg

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